Scientific Reports
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2020
·Vol. 10
·期 1
·1-9
·
IF 3.998
Meng Xianglong,Zhou Pin,Li Lu,Liu Lizhong,Guo Mingming,Sun Tonghua
The selectivity of a facile reductive and extractive desulfurization process was studied. In this desulfurization method, polyethylene glycol was used as the extractant, and sodium borohydride was used as the reductant. Several different simulated fuels were prepared by dissolving thiophenic sulfides, methylbenzene and hexylene in octane. The results showed that methylbenzene and olefins had different effects on different sulfur compounds during this desulfurization process. The extraction and reduction mechanisms were also explained. Four factors could affect the desulfurization performance: (1) intermolecular hydrogen bonding: (a) active O bonding with aromatic H or (b) S bonding with H atoms in hydroxide radicals, (2) “like-dissolves-like” interactions between polyethylene glycol and thiophenic sulfides, (3) the methyl steric hindrance effect and the electron density of sulfur atoms, and (4) the combination of S atoms with produced nickel boride to form active desulfurization centres. The desulfurization reaction path was also deduced according to the GC/MS results.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
PubMed
高影响因子
FUEL
·
2018
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IF 4.908
Hang Xu,Dandan Zhang,Fengmin Wu,Xuefeng Wei,Jun Zhang
Deep eutectic solvents (DESs) are receiving increasing attention as ionic liquid analogues because of their environmentally friendly and very low-price characteristics. In this study, metal-based deep eutectic solvents (MDESs) were synthesized by combining cobalt chloride (CoCl 2 ), a hydrogen bond acceptor (HBA) such as choline chloride (ChCl), and hydrogen bond donors (HBDs) such as polyethylene glycol (PEG-200), ethylene glycol (EG), glycerol (GL), and propionic acid (Pr). The MDESs were used for the extractive catalytic oxidative desulfurization (ECODS) of fuels. Solid peroxymonosulfate (PMS) was selected as an oxidant over common ECODS oxidants such as liquid hydrogen peroxide because the former is cheaper, more stable, and less corrosive. The MDESs played dual roles (i.e., extractant and catalyst) during the ECODS process. One of the MDESs prepared (CoCl 2 -ChCl/2PEG) showed fast reaction rates with nearly 100% dibenzothiophene removal under the optimal conditions (6 g of model oil with an initial sulfur content of 500 ppm, 0.9 g of PMS solution, 2 g of CoCl 2 -ChCl/2PEG, 20 °C, and 60 min). The DESs prepared showed an outstanding recycling performance after 6 cycles without a significant decrease in activity. In the ECODS system, the reactivity of the three sulfur substrates studied followed the order: dibenzothiophene (DBT) > 4,6-dimethyldibenzothiphene (4,6-DMDBT) > benzothiophene (BT). In the case of the HBDs, the desulfurization efficiencies followed the sequence: PEG-200 > Pr > EG > GL. The oxidative product was dibenzothiophene sulfone (DBTO 2 ).
研究领域:
化学工程
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环境科学
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催化材料
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Yizhen Su,Fuquan Xiao,Qibin Yuan,Honglei Zhao,Ruiqi Tang,Linhua Zhu,Chunyan Dai
The development of simple and efficient desulfurization catalysts has garnered increasing attention in the field of desulfurization. In this study, comb-grafted polyethylene phosphomolybdenum-vanadium heteropoly acid catalysts (P-VPA-Mo m V n ) were synthesized via the bulk polymerization method. The structure and morphology of the catalysts were investigated by FTIR, GPC, 1 H NMR, XRD, XPS and SEM. By incorporating ionic liquid as an extractant, the P-VPA-Mo 10 V 2 demonstrates high activity in oxidative desulfurization, removing all DBT from the model oil with a low O/S molar ratio under mild conditions. It is noteworthy that when the reaction temperature is 30 °C, the O/S molar ratio is 3, and the reaction time is 60 min, the catalyst exhibits excellent recycling lifetime of 10 cycles without a significant decline in activity. The incorporation of the ionic liquid further enhances its extraction efficiency, indicating that the catalyst not only possesses a stable structure but also holds strong prospects for industrial application.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2019
·Vol. 9
·期 5
·448
·
IF 3.444
Meng Li,Jinhe Song,Fan Yue,Fan Pan,Wei Yan,Zelin Hua,Long Li,Zhuhong Yang,Licheng Li,Guangming Wen,Kongguo Wu
Mesoporous TiO2containing different potassium content was prepared from potassium titanate by mediating the pH value of the ion exchange, which was used as catalytic support to load NiMo for hydrodesulfurization of dibenzothiophene. The as-prepared samples were characterized by X-ray diffraction, N2physical adsorption/desorption, temperature-programmed reduction, scanning electron microscope/energy dispersive X-ray mapping analysis, high resolution transmission electron microscopy, and pyridine-adsorbed Fourier transform infrared spectroscopy. The characterization results showed that NiO and MoO3were well dispersed on mesoporous TiO2with varying potassium content. A crystal NiMoO4phase was formed on the TiO2with relatively high potassium content, which could decrease the reduction temperature of oxidized active species. The evaluation results from the hydrodesulfurization displayed that as the potassium content of the catalyst increased, the dibenzothiophene conversion firstly increased and then slightly decreased when potassium content exceeded 6.41 wt %. By contrast, the direct desulfurization selectivity could continuously increase along with the potassium content of catalyst. Furthermore, the change in direct desulfurization selectivity of a TiO2-supported NiMo catalyst was independent of the reaction condition. The mesoporous TiO2-supported NiMo catalyst incorporated with potassium could have near both 100% of dibenzothiophene and 100% of direct desulfurization selectivity. According to the structure–performance relationship discussion, the incorporation of potassium species could benefit the formation of more sulfided active species on mesoporous TiO2. Moreover, excessive free potassium species may poison the active sites of the hydrogenation pathway. Both factors determined the characteristics of complete hydrodesulfurization of dibenzothiophene via a direct desulfurization pathway for potassium-incorporated mesoporous TiO2supported NiMo catalysts.Keywords:TiO2;potassium;hydrodesulfurization;dibenzothiophene;direct desulfurization;selectivity
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
DOI
高影响因子
FUEL
·
2016
·
IF 3.611
Chun-feng Mao,Rong-xiang Zhao,Xiu-ping Li
A series of Brønsted-Lewis acidic deep eutectic solvents (DESs) of C 9 H 10 O 2 ·XZnCl 2 (X from 0.5 to 3) were synthesized by simple mixing. The DESs were characterized by infrared spectroscopy, electrospray ionization mass spectrometry, and thermogravimetric analysis. The desulfurization of a model oil was investigated using C 9 H 10 O 2 ·XZnCl 2 as the extraction agent and catalyst, and H 2 O 2 as the oxidant. The effects of the molar ratio of phenylpropanoic acid to zinc chloride, reaction temperature, oxygen to sulfur (O/S) molar ratio, and volume ratio of DESs to oil on the desulfurization rate were investigated. The optimal conditions for desulfurization were determined to be a phenylpropanoic acid to zinc chloride ratio of 2:1, a reaction temperature of 50 °C, an O/S ratio of 6, a DESs to oil volume ratio of 0.25:1, and a model oil dosage of 5 mL. Under the optimal conditions, a desulfurization rate of 99.23% in 80 min was achieved. The recyclability of the DESs was also investigated, and the results showed that the desulfurization rate decreased slightly after five runs. These results demonstrate that C 9 H 10 O 2 ·0.5ZnCl 2 DESs exhibit high desulfurization activity and stability in extraction and oxidation desulfurization systems.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
AUSTRALIAN JOURNAL OF CHEMISTRY
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2016
·Vol. 70
·期 3
·271-279
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IF 1.427
Pengfei Xing,Rongxiang Zhao,Xiuping Li,Xiaohan Gao
The ultra-deep desulfurization of fuel oil has become inevitable for environmental protection. Here, CoWO4/g-C3N4 was used as a catalyst, H2O2 as an oxidant, and 1-ethyl-3-methylimidazolium ethylsulfate ([EMIM][EtSO4], IL) as an extractant for the oxidative desulfurization of model oil. Scanning electron microscopy, FT-IR spectroscopy, N2 adsorption isotherms, and X-ray diffraction were used to confirm the morphology, structure, and properties of the catalysts. The influence of calcination temperature, loading dose of cobalt, amount of H2O2, reaction temperature, and other parameters were investigated. The removal rate of sulfide in model oil could reach 92.9 % at 80°C in 180 min under the optimal operation conditions (V(oil) = 5 mL, T = 80°C, m(catalyst) = 0.03 g, V(H2O2) = 0.4 mL, t = 180 min, V(IL) = 1.0 mL). In addition, the catalyst was reused five times with no significant reduction in the catalytic activity.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Materials
·
2023
·Vol. 16
·期 6
·2343
·
IF 3.4
Bing Wang,Huanyu Chen,Xingguang Hao,Kai Li,Xin Sun,Yuan Li,Ping Ning
Removal of hydrogen sulfide (H2S) from coke oven gas has attracted increasing attention due to economic and environmental concerns. In this study, tannin extract (TE) absorption combined with binuclear sulfonated phthalocyanine cobalt organic polymer (OTS) and binuclear sulfonated phthalocyanine cobalt (PDS) with a fixed bed reactor is used for removal of H2S. The effect of gas flow rate, concentration of H2S, co-existence of organic sulfide compounds and O2were investigated. Then, the effect of total alkalinity content of TE, NaVO3, OTS and PDS was studied in detail. The experimental results demonstrated that 100% H2S conversion could maintain for 13 h at a total alkalinity of 5.0 g/L, TE concentration of 4.0 g/L, NaVO3concentration of 5 g/L, and OTS and PDS concentration of 0.2 g/L and 0.2 g/L, respectively. The OTS and PDS showed synergistic effect on boosting TE desulfurization efficiency. The results provide a new route for the investigation of liquid catalyzed oxidation desulfurization in an efficient and low-cost way.Keywords:coke oven flue gas;flue gas desulfurization;tannin extract desulfurization;polymer
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Lei Dong,Guang Miao,Xiaoling Ren,Neng Liao,Abdul Waqas Anjum,Zhong Li,Jing Xiao
Desulfurization kinetics and regeneration of silica gel-supported TiO2 extrudates were explored for the reactive adsorptive desulfurization (RADS) process in this work. RADS using TiO2/SiO2 extrudates with varied particle sizes was evaluated. The textural and chemical properties of molded adsorbents were well maintained after extrusion, with a negligible decrease (<0.97%) in the desulfurization capacity for 50 ppm low-sulfur diesel. The RADS of trilobed TiO2/SiO2 was well described with a first-order adsorption kinetic model of ln(C) = −9.42 × 10–3t + 3.84, and TiO2/SiO2 extrudates with smaller particle size may provide larger external surface area and shorter diffusion path. The impacts of packing density and weight hour space velocity (WHSV) on fixed-bed dynamic RADS were discussed. The desorption of adsorbed diesel can be well presented by a first-order model, where the total diesel yield of the RADS process reached above 99.5% at a nitrogen purging temperature ≥150 °C. The effects of solvent structure, polarity, and alkalinity on adsorbent regeneration were further illustrated. This work provides an insight into the aspects of kinetics and regeneration of molded adsorbents to pave the way for industrial fixed-bed desulfurization processes.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2020
·
IF 5.006
Si-Wen Li,Wei Wang,Jian-She Zhao
In this work, deep oxidative desulfurization was attained using a new kind MoO 3 modified magnetic catalysts, in which metal organic framework (MOF-199) as supports and the magnetic Fe 3 O 4 added to provide the extra character for increasing practical use value. The characterization of the as-designed catalysts were assessed by FT-IR, XRD, SEM, TPR and XPS analyses. To be noted, various morphologies of MoO 3 were used to form the final products and compared to discuss their influences on the ODS performance in this work. Among them, the Fe@Mo-4@MOF, containing the fibroid MoO 3 , showed an excellent catalytic performance to the ultra-deep oxidative desulfurization in 45 min, which was mainly attributed to the special morphology of MoO 3 , providing the higher contact area with the DBT to increase the ODS efficiency. Moreover, the possible mechanism was proposed to illustrate the ODS process and only slight decrease of DBT removal was observed after 15 recycling times.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2019
·Vol. 14
·期 4
·546-560
·
IF 2.809
Wang Hanlu,Jibrin Idris,Zeng Xingye
Catalysts for the desulfurization of gasoline samples were synthesized via the immobilization of well-dispersed phosphotungstic acid (HPW) on Mobil composition of matter-twenty-two (MWW) zeolite. Characterization results indicated that these catalysts possess a mesoporous structure with the retention of the Keggin structure of immobilized HPW. Relevant reaction parameters influencing sulfur removal were systematically investigated, including HPW loading, catalyst dosage, temperature, initial S-concentration, molar ratio of oxidant to sulfide (O/S), volume ratio of MeCN to model oil (Ext./oil), and sulfide species. The 40 wt-% HPW/MWW catalyst exhibited the highest catalytic activity with 99.6% dibenzothiophene sulfur removal from prepared samples. The 40 wt-% HPW/MWW catalyst was recycled four times and could be easily regenerated. Finally, as an exploratory study, straight-run-gasoline and fluid catalytic cracking gasoline were employed to accurately evaluate the desulfurization performance of 40 wt-% HPW/MWW. Our research provides new insights into the development and application of catalysts for desulfurization of gasoline.
研究领域:
化学工程
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催化材料
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环境科学
✓ 已验证
DOI
高影响因子
ChemNanoMat
·
2021
·Vol. 7
·期 3
·277-283
·
IF 3.154
Jie Wang,Hongqin Ma,Jia Li,Xinyue Luo,Luqi Yu
Graphical Cu(I) decorated 2D black phosphorus nanosheets were synthesized by a ball-milling method . In the process of ball-milling, the bulk black phosphorus was exfoliated into nanosheets under the action of shearing force. Due to the reducibility of black phosphorus, it can react with CuCl 2 to form Cu(I)/BNPSs-n. As the active component of the adsorbent, Cu(I) species can interact with benzothiophene or dibenzothiophene in fuel to achieve the purpose of adsorption desulfurization. In this study, Cu(І) decorated two-dimensional black phosphorus nanosheets (BPNSs) adsorbents were prepared by a ball-milling method, and their adsorption-desorption performances were tested by batch adsorption experiments. The results showed that Cu(ІI) can be completely reduced to Cu(І) without adding any additional reducing agents during the ball-milling process, owing to the ability of black phosphorus to provide electrons to Cu(ІI). Moreover, the produced Cu(І) species were firmly anchored on BPNSs surface through chemical bonds formed between Cu and P atoms, effectively preventing them from aggregating. As the active sites on BPNSs surface, Cu(I) species can adsorb dibenzothiophene or benzothiophene from fuel by forming π-complexation bonds with them. The maximum adsorption capacity of the adsorbent for dibenzothiophene and benzothiophene were 13.16 and 18.02 mg S/g, respectively. Besides, the adsorption desulfurization activity can be recovered well by adopting simple thermal treatment.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Qiang Liu,Bingsi Liu,Qinze Liu,Qiuyue Zhang,Rongnian Xu,Xuanyue Wu,Hong Xia
Refined design of sustainable sorbent demands to tackle the strong dependence for additional mesoporous support and low utilization in hot coal gas desulfurization. Unlike the well-established preparation of loading sorbents supported on zeolites, a vacuum-assisted self-assemble strategy tapping into the ordered channels of walnut wood is proposed to facilely fabricate three-dimensional (3D) (a%Ce–Mn) y Al 2−y O x desulfurizers with anisotropy which provides a desirable macroporosity for rapid diffusion of H 2 S. Benefiting from the inherent straight channle in micron scale, the obtained (8%Ce–Mn) 1.5 Al 0.5 O x presents the highest breakthrough sulfur capacity (289.79 mg g −1 ) and effective utilization (88.42%) at 700 °C. The favorable rapid diffusion of gases in micro/macropores improves greatly the H 2 O-resistance and anti-interference ability of 3D (8%Ce–Mn) 1.5 Al 0.5 O x for high steam and concentration of reducing gas. The fast mass transport in sulfidation reaction at 700 °C is described perfectly by the improved deactivation kinetics model. This study opens a novel design of the ideal 3D desulfurizers with micron porosity inherited from hierarchical architecture of walnut wood for industrialization utilization in the near future.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）